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Sulfur dots–graphene nanohybrid: a metal-free electrocatalyst for efficient N₂-to-NH₃ fixation under ambient conditions

ChenThese authors contributed equally to this work., Hongyu, Zhu, Xiaojuan, Huang, Hong, Wang, Huanbo, Wang, Ting, Zhao, Runbo, Zheng, Hongguo, Asiri, Abdullah M., Luo, Yonglan, Sun, Xuping
Chemical communications 2019 v.55 no.21 pp. 3152-3155
ammonia, carbon dioxide, catalysts, chemical reactions, electrochemistry, electrodes, greenhouse gas emissions, hydrogen, nanohybrids, nitrogen, sulfur
NH₃ is an important chemical with a wide range of applications, but its synthesis mainly relies upon the harsh Haber–Bosch process with huge CO₂ emission. Electrochemical N₂ reduction offers a carbon-neutral process to convert N₂ to NH₃ under ambient conditions, but it requires efficient and stable catalysts to drive the N₂ reduction reaction. Herein, we report that a sulfur dots–graphene nanohybrid acts as a metal-free electrocatalyst for ambient N₂-to-NH₃ conversion with excellent selectivity. When operated in 0.5 M LiClO₄, this electrocatalyst achieves a large NH₃ yield of 28.56 μg h⁻¹ mgcₐₜ.⁻¹ and a high Faradaic efficiency of 7.07% at −0.85 V vs. reversible hydrogen electrode. Notably, it also shows good electrochemical stability.